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  4. Homolytic versus Heterolytic Hydrogen Evolution Reaction Steered by a Steric Effect
 
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2020
Journal Article
Title

Homolytic versus Heterolytic Hydrogen Evolution Reaction Steered by a Steric Effect

Abstract
Several H−H bond forming pathways have been proposed for the hydrogen evolution reaction (HER). Revealing these HER mechanisms is of fundamental importance for the rational design of catalysts and is also extremely challenging. Now, an unparalleled example of switching between homolytic and heterolytic HER mechanisms is reported. Three nickel(II) porphyrins were designed and synthesized with distinct steric effects by introducing bulky amido moieties to ortho‐ or para‐positions of the meso‐phenyl groups. These porphyrins exhibited different catalytic HER behaviors. For these Ni porphyrins, although their 1e‐reduced forms are active to reduce trifluoroacetic acid, the resulting Ni hydrides (depending on the steric effects of porphyrin rings) have different pathways to make H2. Understanding HER processes, especially controllable switching between homolytic and heterolytic H−H bond formation pathways through molecular engineering, is unprecedented in electrocatalysis.
Author(s)
Guo, Xiajun
Wang, Ni
Li, Xialing
Zhang, Zongayo
Zhao, Jianping
Ren, Wanje
Ding, Shuping
Xu, Gelun
Li, Jianfeng
Apfel, Ulf-Peter  
Fraunhofer-Institut für Umwelt-, Sicherheits- und Energietechnik UMSICHT  
Zhang, Wie
Cao, Rui
Journal
Angewandte Chemie. International edition  
Project(s)
RESOLV
Funder
Deutsche Forschungsgemeinschaft DFG  
DOI
10.1002/anie.202002311
Language
English
Fraunhofer-Institut für Umwelt-, Sicherheits- und Energietechnik UMSICHT  
Keyword(s)
  • homolytic / heterolytic processes

  • hydrogen evolution

  • molecular catalysis

  • nickel porphyrins

  • steric effect

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